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Chiral transcription and enantioselective separation have garnered significant research interests and showed potential for a broad range of practical applications. Here, we present a novel and facile strategy for chiral templating and enantiomers resolution by coating metal-ion-mediated l -phenylalanine derivatives (LPF/M) with graphene oxide (GO) via simply mixing. The LPF/M hydrogels precipitate from the liquid by encapsulation of GO through coordination interactions and hydrogen bonds, making heterogeneous transfer and separation possible. The chirality inversion of the internal LPF/M nanostructure could be triggered by different addition of metal ions, which further provides means for controlled chiral transfer of guest molecules on the outer GO surfaces as demonstrated in the transcription of thioflavin T (ThT) and 3-aminopyridine (AP) at the supramolecular level. Changing the metal ions also provides control over enantiomer selectivity with outstanding efficiency and reproducibility, as revealed by the separation of racemic mixtures of phenylanine (>98%), lysine (>96%), and histidine (>97%). In addition, the resultant hybrid materials exhibit excellent environmental stability and reusability (more than 20 times) with significant separation efficiency. More importantly, the GO-coated LPF/M could determine the enantiomeric composition of various chiral substrates. The proposed strategy opens up a promising avenue for practical chiral separation application. Image 1 [ABSTRACT FROM AUTHOR]